Shanghai Key Laboratory of Functional Materials Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, PR China.
Shanghai Key Laboratory of Functional Materials Chemistry, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai, 200237, PR China.
Anal Chim Acta. 2019 Jan 3;1045:123-131. doi: 10.1016/j.aca.2018.09.013. Epub 2018 Sep 11.
In this work, we presented a facile elution-free method for ultrasensitive enrichment of glycopeptides using two kinds of novel Ce-metal-organic frameworks (Ce-MOF) post-modified with hyaluronic acid (Ce-MOF@HA) and glutamic acid (Ce-MOF@Glu). Both of the synthesized materials remained stable in the loading buffer to enrich glycopeptides selectively and degrade in the eluent to release captured glycopeptides. Due to the dissolution of materials, the elution step of the enrichment process is omitted, resulting in an extremely high sensitivity (detection limit, 0.5 fmol/μL). Meanwhile, Ce-MOF@HA and Ce-MOF@Glu also possessed excellent selectivity with molar ratios of IgG and BSA digests being 1:1000 and 1:500, respectively. Noticeably, the practical applicability of the obtained materials was inspected by analyzing the glycopeptides enriched from human serum (2 μL) by nano-LC-MS, in which 434 N-glycopeptides from 182 N-glycoproteins (by Ce-MOF@HA) and 328 N-glycopeptides from 135 N-glycoproteins (by Ce-MOF@Glu) were detected, respectively. This work provides a new method to simplify the process of glycopeptides enrichment and also paves a novel way for the enrichment of trace targets from complex matrices.
在这项工作中，我们提出了一种简便的无洗脱方法，使用两种新型的透明质酸（Ce-MOF@HA）和谷氨酸（Ce-MOF@Glu）修饰的 Ce 金属有机骨架（Ce-MOF）来超灵敏地富集糖肽。这两种合成材料在加载缓冲液中保持稳定，能够选择性地富集糖肽，并在洗脱液中降解以释放捕获的糖肽。由于材料的溶解，省略了富集过程的洗脱步骤，从而实现了极高的灵敏度（检测限为 0.5 fmol/μL）。此外，Ce-MOF@HA 和 Ce-MOF@Glu 还具有出色的选择性，IgG 和 BSA 消化物的摩尔比分别为 1:1000 和 1:500。值得注意的是，通过分析从人血清中富集的糖肽（2 μL）进行纳米 LC-MS 检测，对所获得的材料的实际适用性进行了检验，其中通过 Ce-MOF@HA 检测到 182 种 N-糖蛋白中的 434 种 N-糖肽，通过 Ce-MOF@Glu 检测到 135 种 N-糖蛋白中的 328 种 N-糖肽。这项工作提供了一种简化糖肽富集过程的新方法，也为从复杂基质中富集痕量靶标开辟了新途径。
